Development of sulfur cathode material for Li-S batteries.

Dharmasena, Ruchira

doi:10.18297/etd/341

Cited by 1 publication

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“…Figure shows the open-circuit voltage profile calculated with eqs and for models (a) SC and (b) SC-N and compares it with discharge voltage profiles measured in low-current regimes for the first discharge in SPAN-based Li–S batteries. , A low-current regime guarantees a discharge behavior that approximates the battery’s theoretical voltage in no-load conditions. , Equation calculates the discharge voltage ( V ( n ) vs Li/Li + ) vs the number of lithium atoms added ( n ) based on the difference between lithium metal’s internal energy per atom E bcc (Li) and the change in total internal energy after adding two lithium atoms into the structure ( E total (M/Li n ) – E total (M/Li n –2 )). , The M stands for models SC or SC-N. This equation neglects entropic contributions to the total energy as they are insignificant at room temperature …”

Section: Resultsmentioning

confidence: 99%

“…8,9 A low-current regime guarantees a discharge behavior that approximates the battery's theoretical voltage in no-load conditions. 44,45 Equation 1 calculates the discharge voltage (V(n) vs Li/Li + ) vs the number of lithium atoms added (n) based on the difference between lithium metal's internal energy per atom E bcc (Li) and the change in total internal energy after adding two lithium atoms into the structure (E total (M/Li n ) − E total (M/Li n−2 )). 46,47 The M stands for models SC or SC-N.…”

Section: Discharge Voltage Profiles and Volume Expansionmentioning

confidence: 99%

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Sulfurized Polyacrylonitrile for High-Performance Lithium–Sulfur Batteries: In-Depth Computational Approach Revealing Multiple Sulfur’s Reduction Pathways and Hidden Li⁺ Storage Mechanisms for Extra Discharge Capacity

Beltran

Balbuena

2020

ACS Appl. Mater. Interfaces

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Like no other sulfur host material, polyacrylonitrile-derived sulfurized carbon (SPAN) promises improved electrochemical performance for lithium–sulfur batteries, based on its compatibility with carbonate solvents and ability to prevent self-discharge and shuttle effect. However, a complete understanding of the SPAN’s lithiation mechanism is still missing because its structural features vary widely with synthesis conditions, and its electrochemical performance deviates from elemental sulfur. This study continues our research on the elucidation of the SPAN’s structural characteristics and lithiation mechanisms via computational approaches. Our models reproduce most experimental data regarding carbon’s graphitization level and conjugated ordering, sulfur–carbon covalent bonding, sulfur loading, and elemental composition. Our simulations emulate the discharge voltage observed in experiments for the first discharge, which reveals that sulfur follows multiple reduction pathways based on its interaction with the carbon backbone. Sulfur reduction takes place above 1.0 V vs Li/Li+ mostly in the SPAN-like material, with no long-chain lithium polysulfide formation. Below 1.0 V vs Li/Li+, the backbone’s electrochemical activity occurs via multiple C–Li and N–Li interactions, mostly with edge carbon atoms and pyridinic nitrogen. Moreover, we identify Li+ binding sites throughout the graphitized backbone that might lead to prohibited energy costs for Li+ deintercalation, which may explain the irreversible capacity loss between the first and second discharges. This work improves understanding of lithiation mechanisms in sulfurized carbon, which is useful for rationally designing SPAN synthesis pathways tailored to increase sulfur loading and enhanced electrochemical performance.

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Section: Resultsmentioning

confidence: 99%

Section: Discharge Voltage Profiles and Volume Expansionmentioning

confidence: 99%

Sulfurized Polyacrylonitrile for High-Performance Lithium–Sulfur Batteries: In-Depth Computational Approach Revealing Multiple Sulfur’s Reduction Pathways and Hidden Li⁺ Storage Mechanisms for Extra Discharge Capacity

Beltran

Balbuena

2020

ACS Appl. Mater. Interfaces

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Development of sulfur cathode material for Li-S batteries.

Cited by 1 publication

References 12 publications

Sulfurized Polyacrylonitrile for High-Performance Lithium–Sulfur Batteries: In-Depth Computational Approach Revealing Multiple Sulfur’s Reduction Pathways and Hidden Li⁺ Storage Mechanisms for Extra Discharge Capacity

Sulfurized Polyacrylonitrile for High-Performance Lithium–Sulfur Batteries: In-Depth Computational Approach Revealing Multiple Sulfur’s Reduction Pathways and Hidden Li⁺ Storage Mechanisms for Extra Discharge Capacity

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Development of sulfur cathode material for Li-S batteries.

Cited by 1 publication

References 12 publications

Sulfurized Polyacrylonitrile for High-Performance Lithium–Sulfur Batteries: In-Depth Computational Approach Revealing Multiple Sulfur’s Reduction Pathways and Hidden Li+ Storage Mechanisms for Extra Discharge Capacity

Sulfurized Polyacrylonitrile for High-Performance Lithium–Sulfur Batteries: In-Depth Computational Approach Revealing Multiple Sulfur’s Reduction Pathways and Hidden Li+ Storage Mechanisms for Extra Discharge Capacity

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Sulfurized Polyacrylonitrile for High-Performance Lithium–Sulfur Batteries: In-Depth Computational Approach Revealing Multiple Sulfur’s Reduction Pathways and Hidden Li⁺ Storage Mechanisms for Extra Discharge Capacity

Sulfurized Polyacrylonitrile for High-Performance Lithium–Sulfur Batteries: In-Depth Computational Approach Revealing Multiple Sulfur’s Reduction Pathways and Hidden Li⁺ Storage Mechanisms for Extra Discharge Capacity